Gold recovery from wastewater should be cost-effective, efficient, and environmentally friendly. In this study, adsorbents containing Fe(II,III) systems were prepared via thermal modification of pyrite. The effects of thermal modification temperature, the source of pyrite, pH, ionic strength, adsorbent solid–liquid ratio, and coexisting metal ions on adsorption were investigated. Further, the removability of iron ions was explored, and multiple adsorption–desorption experiments were conducted to verify the stability and recyclability of the adsorbent. The adsorption law and mechanisms were analyzed using adsorption isotherms, thermodynamics, kinetics, and spectroscopy. The results revealed that the natural pyrite modified at 300°C ( N-Py-300) was a more suitable gold adsorbent with a maximum adsorption of 1055.2 mg/g at 25 °C. When coexisting with other metal ions, N-Py-300 exhibited highly selective adsorption of Au(III). Using a mixture of 10 % thiourea and 2 % HCl as a desorbent facilitated the desorption of almost all Au from N-Py-300, resulting in the recovery of Au and the reuse of N-Py-300. The Fe ions released from the adsorbent were effectively reduced by the addition of Ca(OH)₂. The adsorption kinetics and isotherm data were in strong agreement with the pseudo-secondary and Langmuir models, indicating that Au(III) was chemisorbed on N-Py-300 as a monolayer and that Au(III) was reduced to Au(0) and Au(Ⅰ). The pH and IS also affected the adsorption behavior, implying that an electrostatic effect exists. Our findings provide that the thermally modified pyrite can be used to recover precious metals from wastewater efficiently, and provides an experimental basis for the resourceful use of pyrite.